期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 303, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120897
关键词
Covalent-organic frameworks; Electrocatalysis CO2 reduction; NH2-MWCNT; Covalently connection
资金
- National NSFC [22102178, 22178077]
- China Postdoctoral Science Foundation [2021M693119]
- Postdoctoral Scientific Research Starup Project in Heilongjiang Province [LBH-Q19111]
- Natural Science Foundation of Heilongjiang Province [LH2020B013]
- Harbin University of Science and Technology Fund for Distinguished Young Scholars [2019-KYYWF-0213]
By covalently anchoring porphyrin-based COFs nanosheets on carbon nanotubes, efficient electrocatalytic CO2 reduction reactions can be achieved with enhanced activity and selectivity, especially with the formation of copper-based nanoclusters playing a crucial role in improving performance.
Porphyrin-based covalent organic frameworks (Por-COF) nanosheets were vertically anchored on carbon nanotubes (CNT) with covalent connection for efficient electrocatalytic CO2 reduction reaction (CO2RR). The CNT not only acts as ideal carriers for the dispersion of Pro-COF but also facilitates electron transfer along porphyrin planes to immobilized metal active sites. As a result, covalently linked MWCNT-Por-COF-M (M: Co, Ni, Fe) display improved electrocatalytic CO2-to-CO activity and selectivity compared to pure Por-COF-M and MWCNT@Por-COF-M without covalent connection between two components. In particular, MWCNT-Por-COF-Co exhibits superior activity (FECO: 99.3%), higher partial current density and good durability in 0.5 M KHCO3 by H type cell, while MWCNT-Por-COF-Cu exhibits the highest CH4 faradaic efficiency of 71.2% in 1.0 M KOH by flow cell. The results of HRTEM and Auger spectrum revealed that the high performance of MWCNT-Por-COF-Cu could be attributed to the generated Copper-based nanoclusters during the electrocatalytic CO2RR process.
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